Dark oxidation of mercury droplet: Mercurous [Hg(I)] species controls transformation kinetics

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2023-10-01 DOI:10.1016/j.watres.2023.120472

Ying Wang , Guangliang Liu , Yingying Fang , Peng Liu , Yanwei Liu , Yingying Guo , Jianbo Shi , Ligang Hu , Yong Cai , Yongguang Yin , Guibin Jiang

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Abstract

Liquid elemental mercury droplet (Hg(0)_l) is an important species in heavy Hg-contaminated environments. The oxidation processes of Hg(0)_l and its related mechanisms are still poorly understood. Herein, for the first time, it was verified that mercurous species [Hg(I)] was an important species in natural water contaminated by Hg(0)_l as well as in the simulated dark oxidation of Hg(0)_l. The formation and further transformation of Hg(I) controlled the overall oxidation process of Hg(0)_l and were affected by different environmental factors. Through kinetic modeling using ACUCHEM program, oxidation of Hg(0) to Hg(I) (Hg(0) → Hg(I)) was determined to be the rate-limiting step in Hg(0)_l oxidation because its k value ((8.7 ± 0.21) × 10⁻¹¹ s⁻¹) is seven orders of magnitude lower than that of Hg(I) oxidation (Hg(I) → Hg(II), (4.7 ± 0.15) × 10⁻⁴ s⁻¹). Ligands like OH⁻, Cl⁻, and natural organic matter enhanced the formation of Hg(I) via promoting the constants of comproportionation (up to (9.5 ± 0.78) × 10⁻⁴ s⁻¹). These findings highlight the importance of Hg(I) in Hg(0)_l oxidation process by controlling the transformation kinetics of Hg species, facilitating an improved understanding of the environmental redox cycles of Hg.

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汞滴的暗氧化：汞[Hg（I）]物质控制转化动力学。

液态元素汞滴（Hg（0）l）是重汞污染环境中的一个重要物种。Hg（0）l的氧化过程及其相关机制尚不清楚。在此，首次证实了汞物种[Hg（I）]是被Hg（0）l污染的天然水中以及模拟Hg（O）l的暗氧化中的重要物种。Hg（I）的形成和进一步转化控制了Hg（0）l的整个氧化过程，并受到不同环境因素的影响。通过使用ACUCHEM程序进行动力学建模，将Hg（0）氧化为Hg（I）（Hg（0→Hg（I））是Hg（0）l氧化的限速步骤，因为其k值（（8.7±0.21）×→Hg（II），（4.7±0.15）×10-4s-1）。OH-、Cl-和天然有机物等配体通过促进比例常数（高达（9.5±0.78）×10-4s-1）促进了Hg（I）的形成。这些发现通过控制Hg物种的转化动力学，突出了Hg（Ⅰ）在Hg（0）l氧化过程中的重要性，有助于更好地理解汞的环境氧化还原循环。

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来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.